The optoelectronic properties of quantum dots are strongly controlled by the chemical nature of their surface-passivating ligands. In this work, we present the synthesis, characterization, and surface modification of CdSe quantum dots (QDs) and their application in solar cells. CdSe QDs were capped in oleic acid (OA), 3-mercaptopropionic acid (MPA), and 4-mercaptobenzoic acid (MBA). The QDs were characterized by transmission electron microscopy (TEM), UV-Vis absorption and emission spectrophotometry, thermogravimetric analyses, and 1H and 13C NMR. From TEM analysis, it has been observed that interparticle distance can be effectively controlled by the presence of different molecular size ligands. From the 1H and 13C NMR, specific types of interactions between the Cd2+ and the ligands have been observed. Although CdSe/OA presented larger interparticle distance as compared to CdSe/MPA and CdSe/MBA, the photocatalytic oxidation of the thiol groups on the surface of the MPA- and MBA-based quantum dots resulted in poor surface stabilization, ultimately resulting in poor power conversion efficiencies which were ca. 70% smaller than that of OA-based solar cell.
In this work, we show the effect of the thermal treatment temperature on the photoelectrochemical (PEC) activity of CdSe/TiO2 nanocomposites. TiO2 nanotubes (NTs) were synthesized by anodization and the nanocomposites were obtained by depositing CdSe clusters via magnetron sputtering. A two-step thermal treatment was performed: heating the TiO2 NTs at different temperatures prior to CdSe deposition and further heating the CdSe/TiO2 nanocomposites. The nanocomposites were characterized by Rutherford backscattering spectroscopy (RBS), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM), high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), UV-Vis spectrophotometry, and electrochemical impedance spectroscopy (EIS). To compare the PEC performance of the CdSe/TiO2 nanocomposites and pristine TiO2 NTs, linear sweep voltammetry (LSV) curves were obtained under visible light and under 1 sun illumination. It was observed that CdSe incorporation into the TiO2 template enhances the visible light absorbance thereby improving the PEC performance of the nanocomposites. We have found that the optical, structural and PEC properties of the CdSe/TiO2 nanocomposites are dependent on the thermal treatment temperature of the TiO2 nanotubular substrate, prior to CdSe deposition. Moreover, a three-fold improvement in photocurrent was observed upon further thermal treatment of the obtained nanocomposite.
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